Theory-guided design of nanoporous CuMn alloy for efficient electrocatalytic nitrogen reduction to ammonia

Abstract Electrocatalytic nitrogen reduction reaction (NRR) is a highly attractive route for the synthesis of ammonia. However, the efficiency of the electrocatalytic NRR remains low because of the lack of effective catalyst. Here we use density functional theory (DFT) to investigate the effect of alloying Cu with Mn on NRR performance, showing that the incorporation of Mn into Cu structure can greatly improve the NRR performance. Based on the DFT results, we employ a dealloying method to prepare nanoporous CuMn (np-CuMn) alloy as the electrocatalyst for NRR. Thanks to the synergy between Cu and Mn and the nanoporous structure, the as-prepared np-CuMn alloy exhibits a high ammonia yield rate of 28.9 μg h−1 cm−2 with a Faradaic efficiency of 9.83% at −0.3 V versus reversible hydrogen electrode under ambient conditions. Both values are higher than those obtained for most of the reported noble metal catalysts under similar conditions. Our findings offer an opportunity to design high performance NRR catalyst for ammonia synthesis.